Science Advances

Supplementary Materials

This PDF file includes:

  • Section S1. Experimental methods
  • Section S1.1. Sample preparation
  • Section S1.2. 2D IR spectrometer
  • Section S1.3. 3D Fourier transformation
  • Section S1.4. Nonlinear signal pump and probe power dependence
  • Section S2. Supporting results
  • Section S2.1. Transmission and transient pump-probe spectra of uncoupled systems
  • Section S2.2. 2D IR and transient pump-probe spectra and 2D-IR spectral cuts
  • Section S2.3. 2D IR spectra for various molecular concentrations
  • Section S2.4. Early-time dynamics of 2D IR spectral cuts
  • Section S2.5. Two-component spectral fitting of absorptive pump-probe spectra
  • Section S3. Theory
  • Section S3.1. Scaling of polariton nonlinearities
  • Section S3.2. Feynman diagrams for the AC signal
  • Section S3.3. Phenomenological simulation of polariton bleach
  • Section S3.4. Cavity coherence volume
  • Fig. S1. Scheme of 2D IR experimental setup.
  • Fig. S2. 3D FFT frequency domain (ω123) spectra.
  • Fig. S3. IR power dependence.
  • Fig. S4. Linear transmission and pump-probe spectra of uncoupled W(CO)6/hexane systems with 12- and 25-μm cavity longitudinal lengths.
  • Fig. S5. Pump-probe and 2D IR spectra and their spectral cuts at LP/UP pump frequencies.
  • Fig. S6. 2D IR spectra of the 25-μm system at t2 = 0 ps with various concentrations.
  • Fig. S7. Early-time dynamics of 2D IR spectral cuts at ω1 = ωLP/ωDark and AC/DC components of LP/UP cuts between 0 and 6 ps.
  • Fig. S8. Spectral fitting of 25-μm systems with t2 = 0 ps at ω1 = ωLP and ω1 = ωUP.
  • Fig. S9. Feynman diagrams representing the oscillating nonlinear responses (AC components) in each region.
  • Table S1. Parameters of two-component fitting.
  • References (4246)

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